A Pyrene-4,5,9,10-Tetraone-Based Covalent Organic Framework Delivers High Specific Capacity as a Li-Ion Positive Electrode

Hui Gao, Alex R. Neale*, Qiang Zhu, Mounib Bahri, Xue Wang, Haofan Yang, Yongjie Xu, Rob Clowes, Nigel D. Browning, Marc A. Little*, Laurence J. Hardwick*, Andrew I. Cooper*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

82 Citations (Scopus)
16 Downloads (Pure)

Abstract

Electrochemically active covalent organic frameworks (COFs) are promising electrode materials for Li-ion batteries. However, improving the specific capacities of COF-based electrodes requires materials with increased conductivity and a higher concentration of redox-active groups. Here, we designed a series of pyrene-4,5,9,10-tetraone COF (PT-COF) and carbon nanotube (CNT) composites (denoted as PT-COFX, where X = 10, 30, and 50 wt % of CNT) to address these challenges. Among the composites, PT-COF50 achieved a capacity of up to 280 mAh g-1 as normalized to the active COF material at a current density of 200 mA g-1, which is the highest capacity reported for a COF-based composite cathode electrode to date. Furthermore, PT-COF50 exhibited excellent rate performance, delivering a capacity of 229 mAh g-1 at 5000 mA g-1 (18.5C). Using operando Raman microscopy the reversible transformation of the redox-active carbonyl groups of PT-COF was determined, which rationalizes an overall 4 e-/4 Li+ redox process per pyrene-4,5,9,10-tetraone unit, accounting for its superior performance as a Li-ion battery electrode.

Original languageEnglish
Pages (from-to)9434-9442
Number of pages9
JournalJournal of the American Chemical Society
Volume144
Issue number21
Early online date19 May 2022
DOIs
Publication statusPublished - 1 Jun 2022

Keywords

  • porous materials
  • Li-ion batteries
  • electrochemistry
  • Raman spectroscopy
  • composite materials
  • covalent organic frameworks

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